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Letter
Interface States in Bilayer Graphene Encapsulated by Hexagonal Boron Nitride
Kayoung Lee, En-Shao Liu, Kenji Watanabe, Takashi Taniguchi, and Junghyo Nah
ACS Appl. Mater. Interfaces, Just Accepted Manuscript • DOI: 10.1021/acsami.8b16625 • Publication Date (Web): 15 Nov 2018
Downloaded from http://pubs.acs.org on November 16, 2018

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3 Interface States in Bilayer Graphene Encapsulated by Hexagonal Boron Nitride
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6 Kayoung Lee,1,2,* En-Shao Liu,1 Kenji Watanabe,3 Takashi Taniguchi,3 and Junghyo Nah1,4
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8 Microelectronics Research Center, The University of Texas at Austin, Austin, TX 78758 USA
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School of Materials Science and Engineering, Gwangju Institute of Science and Technology,
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Gwangju 61005, South Korea
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15 National Institute for Materials Science, 1-1 Namiki Tsukuba, Ibaraki 305-0044, Japan.
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Department of Electrical Engineering, Chungnam National University, Daejeon 34134,
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South Korea
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22 kayoung.lee@gist.ac.kr
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26 Abstract
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28 The threshold voltages at the onset of conduction for electron and hole branches can
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provide information on band gap values or the interface states in a gap. We measured conductivity
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33 of bilayer graphene encapsulated by hexagonal boron nitride as a function of back and top gates,
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35 where another bilayer graphene is used as a top gate. From the measured conductivity the transport
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gap values were extracted assuming zero interface trap states, and they are close to the theoretically
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40 expected gap values. From a little discrepancy an average density of interface states per energy
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42 within a band gap (Dit) is also estimated. The data clearly show that Dit decreases as a bilayer
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44 graphene band gap increases rather than being constant. Despite the decreasing trend of Dit,
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47 interestingly the total interface states within a gap increases linearly as a band gap increases. This
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49 is because of ~ 2  1010 cm-2 interface states localized at band edges even without a band gap, and
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51 other gap states are equally spread over the gap.
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56 Keywords: bilayer graphene, transport gap, band gap, interface states, hexagonal boron nitride
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3 Bernal stacked bilayer graphene is distinctive from monolayer graphene as the inversion
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6 symmetry can be easily broken via a transverse electric field (E-field)1. The E-field induced on-
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8 site electron energy asymmetry gives rise to a tunable band gap2,3, a variety of quantum Hall
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10 phases4–8, exotic valley transport9,10, etc. Such tunability renders bilayer graphene more promising
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for dynamically tunable device applications. E-field induced band gap of bilayer graphene has
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15 been investigated theoretically and experimentally using various techniques for years. General
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17 picture of band structure of bilayer graphene is understood based on the tight-binding model2,4,11.
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Ab initio density functional theory further confirms the tight-binding idea, but results in stronger
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22 screening of the external interlayer potential yielding a little smaller band gap compared to tight-
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24 binding calculations12,13. Several infrared spectroscopic measurements showed band gap values
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26 as a function of back-gate bias14–16, which agrees well with self-consistent tight-binding14,16 or ab
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29 initio density functional theory calculation15. Temperature (T) dependent measurements at high
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31 E-fields have shown the thermal activation energy approaching half of theoretical band gap
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33 values17–19. But at relatively small E-fields conduction paths through localized states hamper the
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extraction of thermal activation energy20,21. Fermi energy measurement using double bilayer
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38 graphene heterostructures also provided band gap values in agreement with ab initio density
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40 functional theory calculation8.
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Another straightforward measure of a band gap is probing a transport gap. Conduction of
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45 gapped semiconductor is suppressed when its Fermi energy is located inside a gap. A finite gate
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47 bias is required to move Fermi energy to a conduction or valence band edge at which electrical
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49 conduction appears. The threshold bias is thus almost linearly dependent on band gap values. The
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52 transport gap of bilayer graphene on oxide dielectrics was measured at different E-fields using
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54 dual-gated structures22. At a finite E-field, bilayer graphene conductivity shows threshold voltages
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3 along the electron and hole branches, analogous to the threshold voltages seen in a conventional
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6 bulk semiconductor with a band gap. However, the size of the measured transport gap is far larger
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8 than theoretical band gap values because of numerous localized states inside the transport gap.
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10 Here we perform the transport gap measurement on high quality double bilayer graphene
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heterostructures with hexagonal boron nitrides (hBN) dielectrics. hBN provides nearly pristine
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15 environment for graphene and induces negligible localized states and potential fluctuation
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17 compared to oxide dielectrics. We compare our measured transport gap with theoretical gap
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values, and extract interface states in bilayer graphene encapsulated by hBN, providing a detailed
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22 analysis of the variation of gap states as a function of gap size.
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40 Figure 1: (a) A schematic which describes the vertical structure of our device (upper), and a
41 micrograph of sample #1 (lower). (b) Conductivity of sample #1 as a function of VTG
42 and VBG, measured at T = 1.5 K.
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46 Figure 1(a) lower micrograph shows one of our double bilayer graphene heterostructures,
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48 and the upper schematic describes the vertical structure of the device. Samples are fabricated using
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50 a general dry transfer process, elaborated in Ref.8,23. Double bilayer graphene heterostructures can
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be considered as dual-gated bilayer graphene systems using the top bilayer graphene as a top-gate
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55 with relatively low density of states compared to a conventional metal gate. Back-gate bias (VBG)
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3 is applied on the highly degenerate Si substrate, and top-gate bias (VTG) is applied on the top bilayer
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6 graphene. Bottom bilayer graphene conductivity (σ) was measured as a function of VBG and VTG
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8 using a conventional low-current lock-in technique while grounded in average. Figure 1(b) shows
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10 the measured conductivity of the bottom bilayer graphene of sample #1 at T = 1.5 K. Here,
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13 conductivity lower than 0.05 mS is presented as black, which is indeed along the diagonal
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15 charge neutrality line. VBG and VTG control carrier densities of the bottom (nB) and top (nT) bilayer
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17 graphene and corresponding chemical potentials of the bottom (μB) and top (μT) bilayers, as
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20 described by8,24
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22 eVBG = e2(nB + nT)/CBG + μB (1)
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24 eVTG = −e2nT/CTG − μT + μB (2).
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CBG and CTG are capacitances of back-gate and top-gate dielectrics, and e is electron charge. VBG
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29 and VTG in Eqs. (1) and (2) are referenced with respect to the bias values at nB = nT = 0 (double
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31 charge neutrality point, DNP, at which both top and bottom graphene have zero carrier density).
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33 Using a dual-gated structure both carrier density and E-field across the bottom bilayer graphene
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36 (EB) can be independently controlled. EB is given by
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38 EB = enB/2ɛ0 + enT /ɛ0 + EB0 (3)
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40 where EB0 is a built-in E-field in the bottom bilayer graphene at DNP by unintentional doping25,
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43 and ɛ0 is vacuum permittivity. At nB = EB = 0 Eq. (1) and Eq. (3) yield EB0 = −enT /ɛ0 = CBGVBG/ɛ0,
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45 where VBG is the difference between the VBG values at DNP and at the nB = EB = 0 point25. nB =
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EB = 0 point is identified as the charge neutrality point (Dirac point) with a highest conductivity
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50 as marked in Fig. 1(b) [point (i), minimum band gap point], which is expected to have a minimum
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52 band gap. From that point EB increases along the charge neutrality line. We note that in Fig. 1(b)
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3 the black region with a vanishing conductivity gradually increases as EB increases, which means a
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6 higher gate bias is required to gain conductivity at a higher EB.
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Figure 2: (a) nB, (b) nT, and (c) EB calculated as a function of VBG and VTG for sample #1.
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22 Our previous study in double bilayer graphene heterostructures provides a direct chemical
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24 potential measurement technique and measured chemical potential of bilayer graphene as a
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function of carrier density8,24. Using this μ vs n dependence for bilayer graphene Eqs. (1) and (2)
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29 are solved self-consistently and yield carrier density and corresponding chemical potential vs VBG
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31 and VTG. Figure 2(a, b) show the calculated nB and nT, respectively, as a function of VBG and VTG
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33 for sample #1, and Fig. 2(c) presents EB consecutively calculated using nB and nT.
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36 Figure 3(a, b) shows conductivity of the bottom bilayer graphene at different EB values as
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38 a function of nB, measured at T = 1.5 K in samples #1 and #2. Even at EB = 0, σ is non-zero at nB
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40 = 0 [point (i), minimum band gap point] because of thermally excited carriers and disorder in
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43 graphene. By contrast, at a finite E-field σ becomes vanishing at nB = 0 [point (ii)] and remains
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45 vanishing up to a finite threshold |nB| [point (iii)], which increases with the E-field. Sample #2
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47 was measured with more number of data points, and thus threshold points are clearer compared to
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sample #1. Note that here nB denotes the carrier density calculated neglecting band-gaps, rather
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52 than the actual mobile carrier density in gapped graphene. At a non-zero E-field a finite gate bias
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54 is required to move Fermi energy to either a conduction or valence band edge. Therefore,
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3 conductivity of gapped bilayer graphene remains vanishing until applying a finite threshold bias,
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6 VBG′ and VTG′ for VBG and VTG respectively. Such behavior was observed previously in dual-gated
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8 bilayer graphene systems with oxide dielectrics22, but our current systems with hBN dielectric
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10 layers show noticeably reduced threshold |nB|. This is thanks to reduced interface states, and it
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allows us to extract transport gaps (Δ) closer to actual band gap values.
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26 Figure 3: Conductivity of the bottom bilayer graphene as a function of nB at different EB,
27 measured in (a) sample #1 and (b) sample #2, at T = 1.5 K. (c) The extracted transport
28 gap values as a function of an E-field. Transport gaps were measured in the bottom
29 bilayer graphene of sample #1 (blue open) and sample #2 (red open). We also include
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the transport gaps measured in bilayer graphene with oxide dielectrics, Sample A and
32 Sample B, data from Ref.22 (light and dark green), and a gap value in sample #1
33 measured using a chemical potential measurement technique8 (blue closed) for
34 comparison. Dashed line represents theoretically calculated gap values12.
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The transport gap extraction mechanism previously used for dual-gated bilayer graphene
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40 systems with oxide dielectrics22 can be employed for our current system. However, the change of
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42 top graphene chemical potential is considered rigorously here because of low density of states in
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44 graphene. When only VBG′ is applied while keeping VTG constant as the bias value at point (ii),
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47 VBG′ induces the changes in a Si back-gate electron density δnBG , a bottom graphene Fermi level
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49 δ𝜇B_BG, and a top graphene Fermi level δμT_BG. Note that the change in a top graphene electron
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density by VBG′ is then −δnBG because there is no carriers in the bottom bilayer graphene. In the
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54 same manner, when only VTG′ is applied while keeping VBG constant as the bias value at point (ii),
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56 VTG′ induced the changes in a top graphene electron density δnTG , a bottom graphene Fermi level
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3 δμB_TG, and a top graphene Fermi level δμT_TG. Here the change in a back-gate electron density by
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6 VTG′ is then −δnTG . Writing VBG′ (or VTG′) as the sum of changes in Fermi level and electrostatic
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8 potential using Poisson equation yields
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10 – e2 δnBG
11 eVBG ′ = + δ𝜇B_BG (4)
12 CBG
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14 – e2 δnTG
15 eVTG ′ = – δμT_TG + δ𝜇B_TG (5).
16 CTG
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18 Considering electrostatic potential difference between top-gate (or back-gate) and bottom
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20 graphene when VBG′ (or VTG′) is applied using Poisson equation leads to the following relation:
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23 δ𝜇B_BG = – e2 δnBG /CTG + δμT_BG (6)
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25 δ𝜇B_TG = – e2 δnTG /CBG (7).
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Eqs. (4) and (5) can be then converted into
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30 CTG (δ𝜇B_BG – δ𝜇T_BG )
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CBG
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CBG δ𝜇B_TG
eVTG ′ = – δ𝜇T_TG + δ𝜇B_TG (9)
35 CTG
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37 Using δ𝜇B_BG + δ𝜇B_TG = Δ/2 we obtain the transport gap
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40 2e 2CTG
Δ= (CBG VBG ′ + CTG VTG ′) + (δ𝜇T_BG + δ𝜇T_TG ) (10)
41 CBG + CTG CBG + CTG
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43 Here, any disorder induced interface states are not considered. Figure 3(c) shows the extracted
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46 transport gap values for samples #1 and #2. The sample #1 gap data probed using our another
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48 chemical potential probing technique8 are also included, which can be done only at DNP. The
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50 transport gap values measured in samples #1 and #2 are surprisingly close to the theoretically
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53 expected gap values (dashed line)12. Multiple wide-range temperature dependent
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55 measurements17,18,20,21 were performed to extract thermal activation energies, but only at an E-field
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3 higher than 0.5 V/nm valid gap values were produced. Infrared spectroscopy15,16 provided band
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6 gap values, which is in agreement with theoretical tight-binding calculation, but the number of
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10 In Fig. 3(c) we also show the transport gap measurement data performed on bilayer
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graphene with oxide dielectrics (Samples A and B)22. Samples A and B are on SiO2 substrate and
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15 encapsulated by Al2O3. The transport gaps extracted from the samples with oxide dielectrics are
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17 significantly larger than the theoretical values. This feature is a clear distinction from that of
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samples #1 and #2, bilayer graphene with hBN dielectrics. SiO2 substrates induce spatial disorder
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22 and numerous impurities in graphene resulting in interface trap states within a gap17,20,26–28. Those
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24 gap states should be filled up first to induce carriers in a conduction or valence band, which
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26 requires additional bias across the dielectric. In contrast, the transport gaps measured in sample
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29 #2 with hBN dielectrics agrees very well with the theoretical expectation, showing negligible
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31 disorder and gap states. This confirms that encapsulating graphene with hBN protects the pristine
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33 quality of graphene and presumably general two-dimensional materials as well.
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48 Figure 4: (a) Dit (left axis) and total gap states, Dit, (right axis) extracted from transport gap data
49 of bilayer graphene with oxide dielectrics22 as a function of theoretical gap values for
50 an applied E-field. Closed and open symbols mark Samples A and B respectively. (b)
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52 Dit (left axis) and Dit (right axis) extracted for sample #1. Closed and open symbols
53 represent two opposite E-field directions.
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3 Sample #1 has transport gap values slightly larger than the calculation, and we extracted
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6 the information about gap states from a little discrepancy. Taking into account the density of gap
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8 states in bilayer graphene, Eq. (8) and Eq. (9) are corrected into
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10 CTG (δ𝜇B_BG – δ𝜇T_BG ) e2 Dit δ𝜇B_BG
11 eVBG ′ = + + δμB_BG (11)
12 CBG CBG
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14 CBG δ𝜇B_TG e2 Dit δ𝜇B_BG
15 eVTG ′ = + – δ𝜇T_TG + δ𝜇B_TG (12)
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18 where Dit is average density of gap states per energy. Then the corrected transport gap is given as
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20 2e(CBG VBG ′ + CTG VTG ′ ) + 2CTG (δ𝜇T_BG + δ𝜇T_TG )
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22 CBG + CTG + e2 Dit
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24 By equating Δ to the theoretically calculated gap value and using Dit as a fitting parameter, we
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26 extract Dit as a function of an applied E-field. Figure 4(a) shows the calculated Dit and total gap
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29 states Dit   for Sample A and B, bilayer graphene with oxide dielectrics, as a function of
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31 theoretical gap value. The obtained Dit values vary from 6  1012 to 9  1012 cm-2/eV, and a band
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gap (E-field) dependence is not observed. This gap-size-independent Dit indeed leads to the
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36 linearly increasing total gap-states as a band gap increases as shown in Fig. 4(a). The linear fit
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38 yields averaged Dit = 7.3  1012 cm-2/eV. Fig. 4(b) shows the Dit and total gap states extracted
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from sample #1 as a function of band gap. Interestingly, the extracted Dit in sample #1 decreases
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43 as a band gap increases, distinctive from the behavior seen in samples with oxide dielectrics. This
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45 suggests that Dit is mostly concentrated at a certain energy range, presumably near the band edges.
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Despite the decreasing trend of Dit with an increasing band gap, interestingly the total interface
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50 states in a gap shows a clear linearity with an increasing band gap. The linear fit to the total
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52 interface states vs gap provides a gap state increasing rate as 7.8  1011 cm-2/eV with an intercept
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55 of ~ 2  1010 cm-2 at zero band gap. The standard error of the extrapolated intercept value is ~ 1 
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109 cm-2. This reveals ~ 2  1010 cm-2 interface states localized at band edges even without a band
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6 gap, and 7.8  1011 cm-2/eV density of gap states per energy equally spread over the gap regardless
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8 of the gap size. The intercept values from Fig. 4(a) data are ~ 6  109 cm-2 and ~ 6  1010 cm-2 for
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11 Samples A and B respectively both with a standard error of ~ 4  1010 cm-2, comparable to the
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13 intercept value. This suggests that the density of interface states localized at band edges of samples
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with oxide dielectrics can range up to 1011 cm-2. Several studies17,20,29 provide the estimation of
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18 charge density in fluctuating potentials (puddles), which is in the range of 2  1011 ~ 1012 cm-2 for
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20 graphene on SiO2 and ~ 2  109 cm-2 for graphene on hBN. However, there have been no detailed
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23 study showing the variation of gap states as a function of gap size and the density of interface
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25 states localized at band edges.
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27 In summary, we measured conductivity of bilayer graphene encapsulated by hBN as a
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function of carrier density and transverse E-field. Similar to dual-gated bilayer graphene with
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32 oxides as dielectrics, our samples show finite threshold voltages for the onset of conduction, which
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34 increase as the E-field increases. Surprisingly, the extracted transport gaps are far closer to the
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theoretically expected gap values, in contrast to those of graphene on oxide dielectrics. This
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39 confirms that encapsulating graphene with hBN protects the pristine quality of graphene and
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41 presumably general two-dimensional materials as well. Our study also suggests that our simple
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43 transport gap measurement method is reliable and can be utilized to probe a band gap of other high
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46 quality semiconductors or to extract rich information about interface states.
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3 Acknowledgements
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6 This work was supported by NRI-SWAN. K. L. acknowledges support from the Korean
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8 National Research Foundation (NRF) funded by the Korea government (MSIT) with the grant
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10 number NRF-2018R1C1B3002733 and NRF-2013M3A6B1078873.
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3 References
4
5
6
7 (1) Castro Neto, A. H.; Guinea, F.; Peres, N. M. R.; Novoselov, K. S.; Geim, A. K. The
8 Electronic Properties of Graphene. Rev. Mod. Phys. 2009, 81 (1), 109–162.
9 (2) McCann, E. Asymmetry Gap in the Electronic Band Structure of Bilayer Graphene. Phys.
10 Rev. B 2006, 74 (16), 161403.
11 (3) Castro, E. V.; Novoselov, K. S.; Morozov, S. V.; Peres, N. M. R.; dos Santos, J. M. B. L.;
12
13
Nilsson, J.; Guinea, F.; Geim, A. K.; Neto, A. H. C. Biased Bilayer Graphene:
14 Semiconductor with a Gap Tunable by the Electric Field Effect. Phys. Rev. Lett. 2007, 99
15 (21), 216802.
16 (4) McCann, E.; Fal’ko, V. I. Landau-Level Degeneracy and Quantum Hall Effect in a
17 Graphite Bilayer. Phys. Rev. Lett. 2006, 96 (8), 086805.
18 (5) Maher, P.; Wang, L.; Gao, Y.; Forsythe, C.; Taniguchi, T.; Watanabe, K.; Abanin, D.;
19
Papić, Z.; Cadden-Zimansky, P.; Hone, J.; et al. Tunable Fractional Quantum Hall Phases
20
21 in Bilayer Graphene. Science 2014, 345 (6192), 61–64.
22 (6) Kou, A.; Feldman, B. E.; Levin, A. J.; Halperin, B. I.; Watanabe, K.; Taniguchi, T.;
23 Yacoby, A. Electron-Hole Asymmetric Integer and Fractional Quantum Hall Effect in
24 Bilayer Graphene. Science 2014, 345 (6192), 55–57.
25 (7) Lee, K.; Kim, S.; Points, M. S.; Beechem, T. E.; Ohta, T.; Tutuc, E. Magnetotransport
26 Properties of Quasi-Free-Standing Epitaxial Graphene Bilayer on SiC: Evidence for
27
Bernal Stacking. Nano Lett. 2011, 11 (9), 3624–3628.
28
29 (8) Lee, K.; Fallahazad, B.; Xue, J.; Dillen, D. C.; Kim, K.; Taniguchi, T.; Watanabe, K.;
30 Tutuc, E. Chemical Potential and Quantum Hall Ferromagnetism in Bilayer Graphene.
31 Science 2014, 345 (6192), 58–61.
32 (9) Shimazaki, Y.; Yamamoto, M.; Borzenets, I. V.; Watanabe, K.; Taniguchi, T.; Tarucha, S.
33 Generation and Detection of Pure Valley Current by Electrically Induced Berry Curvature
34 in Bilayer Graphene. Nat. Phys. 2015, 11 (12), 1032–1036.
35
36
(10) Sui, M.; Chen, G.; Ma, L.; Shan, W.-Y.; Tian, D.; Watanabe, K.; Taniguchi, T.; Jin, X.;
37 Yao, W.; Xiao, D.; et al. Gate-Tunable Topological Valley Transport in Bilayer Graphene.
38 Nat. Phys. 2015, 11 (12), 1027–1031.
39 (11) Zhang, L. M.; Li, Z. Q.; Basov, D. N.; Fogler, M. M.; Hao, Z.; Martin, M. C.
40 Determination of the Electronic Structure of Bilayer Graphene from Infrared
41 Spectroscopy. Phys. Rev. B 2008, 78 (23), 235408.
42
(12) Min, H.; Sahu, B.; Banerjee, S. K.; MacDonald, A. H. Ab Initio Theory of Gate Induced
43
44 Gaps in Graphene Bilayers. Phys. Rev. B 2007, 75 (15).
45 (13) Gava, P.; Lazzeri, M.; Saitta, A. M.; Mauri, F. Ab Initio Study of Gap Opening and
46 Screening Effects in Gated Bilayer Graphene. Phys. Rev. B 2009, 79 (16), 165431.
47 (14) Mak, K. F.; Lui, C. H.; Shan, J.; Heinz, T. F. Observation of an Electric-Field-Induced
48 Band Gap in Bilayer Graphene by Infrared Spectroscopy. Phys. Rev. Lett. 2009, 102 (25),
49 256405.
50
(15) Kuzmenko, A. B.; Crassee, I.; van der Marel, D.; Blake, P.; Novoselov, K. S.
51
52 Determination of the Gate-Tunable Band Gap and Tight-Binding Parameters in Bilayer
53 Graphene Using Infrared Spectroscopy. Phys. Rev. B 2009, 80 (16), 165406.
54
55
56
57
58
59
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Page 13 of 14 ACS Applied Materials & Interfaces

1
2
3 (16) Zhang, Y.; Tang, T.-T.; Girit, C.; Hao, Z.; Martin, M. C.; Zettl, A.; Crommie, M. F.; Shen,
4
Y. R.; Wang, F. Direct Observation of a Widely Tunable Bandgap in Bilayer Graphene.
5
6 Nature 2009, 459 (7248), 820–823.
7 (17) Zou, K.; Zhu, J. Transport in Gapped Bilayer Graphene: The Role of Potential
8 Fluctuations. Phys. Rev. B 2010, 82 (8), 081407.
9 (18) Miyazaki, H.; Tsukagoshi, K.; Kanda, A.; Otani, M.; Okada, S. Influence of Disorder on
10 Conductance in Bilayer Graphene under Perpendicular Electric Field. Nano Lett. 2010, 10
11 (10), 3888–3892.
12
13
(19) Yan, J.; Fuhrer, M. S. Charge Transport in Dual Gated Bilayer Graphene with Corbino
14 Geometry. Nano Lett. 2010, 10 (11), 4521–4525.
15 (20) Taychatanapat, T.; Jarillo-Herrero, P. Electronic Transport in Dual-Gated Bilayer
16 Graphene at Large Displacement Fields. Phys. Rev. Lett. 2010, 105 (16), 166601.
17 (21) Oostinga, J. B.; Heersche, H. B.; Liu, X.; Morpurgo, A. F.; Vandersypen, L. M. K. Gate-
18 Induced Insulating State in Bilayer Graphene Devices. Nat. Mater. 2008, 7 (2), 151–157.
19
(22) Lee, K.; Fallahazad, B.; Min, H.; Tutuc, E. Transport Gap in Dual-Gated Graphene
20
21 Bilayers Using Oxides as Dielectrics. IEEE Trans. Electron Devices 2013, 60 (1), 103–
22 108.
23 (23) Dean, C. R.; Young, A. F.; Meric, I.; Lee, C.; Wang, L.; Sorgenfrei, S.; Watanabe, K.;
24 Taniguchi, T.; Kim, P.; Shepard, K. L.; et al. Boron Nitride Substrates for High-Quality
25 Graphene Electronics. Nat. Nanotechnol. 2010, 5 (10), 722–726.
26 (24) Lee, K.; Jung, J.; Fallahazad, B.; Tutuc, E. Transport Spectroscopy in Bilayer Graphene
27
Using Double Layer Heterostructures. 2D Mater. 2017, 4 (3), 035018.
28
29 (25) Fallahazad, B.; Lee, K.; Kang, S.; Xue, J.; Larentis, S.; Corbet, C.; Kim, K.; Movva, H. C.
30 P.; Taniguchi, T.; Watanabe, K.; et al. Gate-Tunable Resonant Tunneling in Double
31 Bilayer Graphene Heterostructures. Nano Lett. 2015, 15 (1), 428–433.
32 (26) Hobbs, C. C.; Fonseca, L. R. C.; Knizhnik, A.; Dhandapani, V.; Samavedam, S. B.;
33 Taylor, W. J.; Grant, J. M.; Dip, L. G.; Triyoso, D. H.; Hegde, R. I.; et al. Fermi-Level
34 Pinning at the Polysilicon/Metal Oxide Interface-Part I. IEEE Trans. Electron Devices
35
36
2004, 51 (6), 971–977.
37 (27) Hobbs, C. C.; Fonseca, L. R. C.; Knizhnik, A.; Dhandapani, V.; Samavedam, S. B.;
38 Taylor, W. J.; Grant, J. M.; Dip, L. G.; Triyoso, D. H.; Hegde, R. I.; et al. Fermi-Level
39 Pinning at the Polysilicon/Metal-Oxide Interface-Part II. IEEE Trans. Electron Devices
40 2004, 51 (6), 978–984.
41 (28) Hobbs, C.; Fonseca, L.; Dhandapani, V.; Samavedam, S.; Taylor, B.; Grant, J.; Dip, L.;
42
Triyoso, D.; Hegde, R.; Gilmer, D.; et al. Fermi Level Pinning at the PolySi/Metal Oxide
43
44 Interface. In 2003 Symposium on VLSI Technology, 2003. Digest of Technical Papers;
45 2003; pp 9–10.
46 (29) Xue, J.; Sanchez-Yamagishi, J.; Bulmash, D.; Jacquod, P.; Deshpande, A.; Watanabe, K.;
47 Taniguchi, T.; Jarillo-Herrero, P.; LeRoy, B. J. Scanning Tunnelling Microscopy and
48 Spectroscopy of Ultra-Flat Graphene on Hexagonal Boron Nitride. Nat. Mater. 2011, 10
49 (4), 282–285.
50
51
52
53
54
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